A new catalytically active zeolite, designated , with a three-dimensional (3D) 11 × 10 × 10-ring topology has been discovered from high throughput experiments while evaluating a family of new organic structure directing agents (OSDAs), 1-alkyl-4-(pyrrolidin-1-yl)pyridin-1-ium hydroxide. The framework structure was determined by model building techniques and confirmed by diffraction calculations. The EMM-17 structure is a random intergrowth of two polymorphs which have a 3D arrangement of intersecting 11 × 10 × 10-ring pores. EMM-17 is stable to calcination to remove the OSDA and can be reproducibly synthesized in the presence of fluoride using common, inexpensive reagents over a wide Si/Al range from 15 to infinity, enabling the catalyst acidity to be tailored to almost any petrochemical application. Unlike OSDAs for many new zeolite structures, the OSDAs for EMM-17 are prepared in one simple alkylation step, making EMM-17 an easy to prepare, highly accessible, catalytically active zeolite. Zeolites containing odd numbered channel sizes are rare, and this is the first confirmed example of a 3D 11-ring aluminosilicate zeolite with a pore size in between those of the commercially important 10-and 12-ring zeolites such as ZSM-5 and Zeolite-Y, respectively. Catalysts prepared from EMM-17 exhibit significantly higher activity for catalytic isomerization with no loss in selectivity than current state of the art catalysts. Catalytic isomerization of linear to branched alkanes is a critical component of commercial dewaxing, allowing for the improvement of cold flow properties of hydrocarbon fuels and lubricants through selective hydroisomerization of normal paraffins.
The selective detection of hydrocarbons using portable microsensors remains a fundamental challenge in materials and microsystem development. This work describes the functioning of a proposed thermoelectric catalytic microsensor using a metal oxide catalyst and a selective partial oxidation reaction for ethanol detection in complex hydrocarbon mixtures containing hundreds of hydrocarbons present in gasoline fuel. In the case where the competing hydrocarbons are nonreactive, 100% selectivity toward ethanol would be obtained and quantification is straightforwardthis case is simulated using ethanol in an inert atmosphere. As an example of detection and quantification in the presence of other reactants, a two step detection sequence is presented for the identification of ethanol concentrations in a hydrocarbon mixture containing methanol. Two-dimensional COMSOL simulations are performed, using known kinetic parameters for ethanol and methanol partial oxidation to acetaldehyde and formaldehyde, respectively, over the chosen iron molybdate catalyst at 353 K, to characterize temperature and concentration profiles within the microelectric thermal sensor/catalytic microreactor, which in turn can be used as a database for a genetic search algorithm used in a real device under unknown environments. Additionally, the knowledge of expected temperature profiles allows one to optimize design parameters for the device to maximize sensor sensitivity and performance for ethanol/methanol verification in complex mixtures.
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